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Long-range intermolecular forces are able to steer polar molecules submergedin superfluid helium nanodroplets into highly polar metastable configurations.We demonstrate that the presence of such special structures can be identified,in a direct and determinative way, by electrostatic deflection of the dopednanodroplet beam. The measurement also establishes the structures' electricdipole moments. In consequence, the introduced approach is complementary tospectroscopic studies of low-temperature molecular assembly reactions. It isenabled by the fact that within the cold superfluid matrix the moleculardipoles become nearly completely oriented by the applied electric field. As aresult, the massive (tens of thousands of helium atoms) nanodroplets undergosignificant deflections. The method is illustrated here by an application todimers and trimers of dimethyl sulfoxide (DMSO) molecules. We interpret theexperimental results with ab initio theory, mapping the potential energysurface of DMSO complexes and simulating their low temperature aggregationdynamics.

Direct detection of polar structure formation in helium nanodroplets by beam deflection measurements